Direct observation of collective modes coupled to molecular orbital–driven charge transfer
2015; American Association for the Advancement of Science; Volume: 350; Issue: 6267 Linguagem: Inglês
10.1126/science.aab3480
ISSN1095-9203
AutoresT. Ishikawa, Stuart A. Hayes, Sercan Keskin, Gastón Corthey, Masaki Hada, Kostyantyn Pichugin, Alexander Marx, Julian Hirscht, Kenta Shionuma, Ken Onda, Y. Okimoto, Shin‐ya Koshihara, Takashi Yamamoto, HengBo Cui, Mitsushiro Nomura, Y. Oshima, M. Abdel-Jawad, Reìzo Kato, R. J. Dwayne Miller,
Tópico(s)Photochemistry and Electron Transfer Studies
ResumoCorrelated electron systems can undergo ultrafast photoinduced phase transitions involving concerted transformations of electronic and lattice structure. Understanding these phenomena requires identifying the key structural modes that couple to the electronic states. We report the ultrafast photoresponse of the molecular crystal Me4P[Pt(dmit)2]2, which exhibits a photoinduced charge transfer similar to transitions between thermally accessible states, and demonstrate how femtosecond electron diffraction can be applied to directly observe the associated molecular motions. Even for such a complex system, the key large-amplitude modes can be identified by eye and involve a dimer expansion and a librational mode. The dynamics are consistent with the time-resolved optical study, revealing how the electronic, molecular, and lattice structures together facilitate ultrafast switching of the state.
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